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Narita, Hirokazu*; Maeda, Motoki*; Tokoro, Chiharu*; Suzuki, Tomoya*; Tanaka, Mikiya*; Shiwaku, Hideaki; Yaita, Tsuyoshi
RSC Advances (Internet), 13(25), p.17001 - 17007, 2023/06
Times Cited Count:1 Percentile:51.1(Chemistry, Multidisciplinary)no abstracts in English
Suzuki, Tomoya*; Otsubo, Ukyo*; Ogata, Takeshi*; Shiwaku, Hideaki; Kobayashi, Toru; Yaita, Tsuyoshi; Matsuoka, Mitsuaki*; Murayama, Norihiro*; Narita, Hirokazu*
Separation and Purification Technology, 308, p.122943_1 - 122943_7, 2023/03
Times Cited Count:2 Percentile:24.43(Engineering, Chemical)HNO leaching is used in recycling Pd metal from spent products that primarily contain Ag, and most Pd residues are separated from solutions containing Ag(I). However, a small amount of Pd(II) often remains in these Ag(I) solutions. Therefore, the separation of Pd(II) and Ag(I) in HNO solutions is essential to promote efficient Pd recycling. In this study, the separation of Pd(II) and Ag(I) in HNO solutions was investigated using four N-donor-type adsorbents functionalized with amine (R-Amine), iminodiacetic acid (R-IDA), pyridine (R-Py), or bis-picolylamine (R-BPA). R-Amine, R-IDA, and R-Py selectively adsorbed Pd(II) over Ag(I), Cu(II), Ni(II), and Fe(III) from HNO solutions (0.3-7 M), but R-Amine exhibited a lower Pd adsorption efficiency. In contrast, 90% of Pd(II), Ag(I), and Cu(II) were adsorbed by R-BPA over the entire range of HNO concentrations. Structural analyses of the adsorbed metal ions using Fourier transform infrared spectroscopy and extended X-ray absorption fine structure spectroscopy revealed the separation mechanisms of the N-donor-type adsorbents. Pd(II) adsorption on R-IDA, R-Py, and R-BPA occurred via Pd(II) coordination of the functional groups (iminodiacetic acid, pyridine, and bis-picolylamine, respectively), whereas that on R-Amine occurred via anion exchange of NO with [Pd(NO)]. The coordinative adsorption mechanisms resulted in the higher Pd(II) adsorption behaviors of R-IDA, R-Py, and R-BPA. HCl (5.0 M) and thiourea (0.1 M) eluents desorbed 83% of Pd(II) from R-IDA and 95% from R-Py, respectively. R-Py was the most effective Pd(II) adsorbent based on adsorption selectivity and desorption efficiency.
Suzuki, Tomoya*; Otsubo, Ukyo*; Ogata, Takeshi*; Shiwaku, Hideaki; Kobayashi, Toru; Yaita, Tsuyoshi; Matsuoka, Mitsuaki*; Murayama, Norihiro*; Narita, Hirokazu*
Dalton Transactions (Internet), 50(33), p.11390 - 11397, 2021/09
Times Cited Count:2 Percentile:21.56(Chemistry, Inorganic & Nuclear)no abstracts in English
Narita, Hirokazu*; Kasuya, Ryo*; Suzuki, Tomoya*; Motokawa, Ryuhei; Tanaka, Mikiya*
Encyclopedia of Inorganic and Bioinorganic Chemistry (Internet), 28 Pages, 2020/12
Suzuki, Tomoya*; Ogata, Takeshi*; Tanaka, Mikiya*; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi; Narita, Hirokazu*
Analytical Sciences, 35(12), p.1353 - 1360, 2019/12
Times Cited Count:3 Percentile:12.45(Chemistry, Analytical)no abstracts in English
Suzuki, Tomoya*; Narita, Hirokazu*; Ogata, Takeshi*; Suzuki, Hideya; Matsumura, Tatsuro; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi
Solvent Extraction Research and Development, Japan, 26(1), p.11 - 19, 2019/06
Times Cited Count:3 Percentile:14.02(Chemistry, Multidisciplinary)The ability of AMP03, a styrene-divinylbenzene copolymer functionalized with -trimethylglycine moieties, to adsorb Pd(II) from HNO solutions was investigated to elucidate the affinity of -trimethylglycine for Pd(II). In the present study, we investigated the mechanism of Pd(II) adsorption by AMP03 by means of adsorption experiments, Fourier Transform Infrared (FT-IR) spectroscopy, and Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy.
Suzuki, Tomoya*; Ogata, Takeshi*; Tanaka, Mikiya*; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi; Narita, Hirokazu*
Metals, 8(7), p.558_1 - 558_10, 2018/07
Times Cited Count:12 Percentile:53.94(Materials Science, Multidisciplinary)The refining of platinum group metals is based mainly on solvent extraction methods, whereas Ru is selectively recovered by distillation as RuO. Replacement of distillation byextraction is expected to simplify the purification process. To develop an effective extraction system for Ru, we analyzed the Ru species in HCl with UV-Vis and EXAFS spectroscopies, and we examined the properties of Ru extracted with N-2-ethylhexyl-bis(N-di-2-ethylhexyl-ethylamide) amine (EHBAA). EXAFS and UV-Vis spectra of Ru in HCl solutions revealed that the predominant Ru species in 0.5-10 M HCl solutions changed from [RuCl(HO)] to [RuCl] with the HCl concentration. The extraction percentages of Ru in the EHBAA system increased with increasing HCl concentration, reached 80% at [HCl] = 5 M, and decreased athigher HCl concentrations. EXAFS analysis of the extracted complex indicated that the Ru had 5 Cl and 1 HO in its inner coordination sphere. The similarity of the dependence on HCl concentrations of the extraction in the EHBAA system and the distribution profile of [RuCl(HO)] on [RuCl(HO)] suggested that the EHBAA extracted the pentachlorido species.
Narita, Hirokazu*; Maeda, Motoki*; Tokoro, Chiharu*; Suzuki, Tomoya*; Tanaka, Mikiya*; Motokawa, Ryuhei; Shiwaku, Hideaki; Yaita, Tsuyoshi
Analytical Sciences, 33(11), p.1305 - 1309, 2017/11
Times Cited Count:11 Percentile:40.7(Chemistry, Analytical)Narita, Hirokazu*; Suzuki, Tomoya*; Motokawa, Ryuhei
Nihon Kinzoku Gakkai-Shi, 81(4), p.157 - 167, 2017/04
Times Cited Count:17 Percentile:62.95(Metallurgy & Metallurgical Engineering)Suzuki, Tomoya; Morita, Keisuke; Sasaki, Yuji; Matsumura, Tatsuro
Separation Science and Technology, 51(17), p.2815 - 2822, 2016/09
Times Cited Count:7 Percentile:23.23(Chemistry, Multidisciplinary)To understand the adsorption properties of styrene-divinylbenzene copolymer functionalized with -trimethylglycine, AMP03, the adsorption behaviors for platinoid ions (Ru(III), Rh(III), and Pd(II)) were examined. Furthermore, we performed adsorption experiments using sample solutions with adding triethylamine, thiourea, and -trimethylglycine. Based on the adsorption data obtained in this study, we performed chromatographic experiments. The results indicated that all platinoid ions in the feed solution completely adsorbed on AMP03, and almost 80% of the adsorbed platinoid ions were recovered. These results show that AMP03 has the potential to recover Ru(III), Rh(III), and Pd(II) from high-level liquid waste.
Suzuki, Tomoya; Morita, Keisuke; Sasaki, Yuji; Matsumura, Tatsuro
Bulletin of the Chemical Society of Japan, 89(5), p.608 - 616, 2016/05
Times Cited Count:5 Percentile:16.1(Chemistry, Multidisciplinary)In a previous study, we found that AMP03 adsorbs Rh(III) from the HNO solution with pH = 1.7 - 2.2. In this study, to understand the Rh(III) adsorption properties of AMP03 and clarify conditions for efficient recovery, we investigated the adsorption behaviors of Rh(III) from the HNO solution. As a result, it was found that Rh(III) is effectively adsorbed from aqueous solution containing low H and high NO concentration. Considering the adsorption mechanism of Rh(III), we found that Rh in aqueous solution is adsorbed with two betaine groups in AMP03 and three NO.
Sasaki, Yuji; Suzuki, Tomoya; Morita, Keisuke; Yoshizuka, Kazuharu*
Hydrometallurgy, 159, p.107 - 109, 2016/01
Times Cited Count:5 Percentile:27.46(Metallurgy & Metallurgical Engineering)The novel tridentate extractant including soft donor has developed and examined. The extractant, tetraoctyl-thiodiglycolamide (S-DGA), is analogous structure to tetraoctyl-diglycolamide (TODGA), but with sulfur donor instead of ether oxygen of TODGA. S-DGA has unique property to extract silver from acidic solutions to n-dodecane with relatively high D values. We investigated the extraction behavior of Ag in various acids, HNO, HSO, and HClO.
Sasaki, Yuji; Tsubata, Yasuhiro; Shirasu, Noriko; Morita, Keisuke; Suzuki, Tomoya
Nihon Genshiryoku Gakkai Wabun Rombunshi, 14(3), p.202 - 212, 2015/09
We have been developing the new partitioning method of high-level radioactive waste by single-cycle extraction process. This process is composed of extraction of actinides (An) and fission products (FP, e.g., Pd, Ru, Mo and Tc), and mutual separation by back-extraction. The extractant employed in this process is required to extract soft, hard acid metals and oxonium anions simultaneously. The NTAamide (hexaoctyl-nitrilotriacetamide) is one of the candidate extractants. After extraction of An and FP, the mutual separation by back-extraction should be set up. Pd and Ru extracted by NTAamide can be back-extracted by complexing agents such as thiourea, systeine, diethylenetriamine, and trisaminoethylamine, and the back-extraction of Mo can be performed by methylimino-diethylacetamide (MIDEA), NTAamide(C2) and iminodimethylphosphoric acid, and Re can be done by aqueous phase with high pH.
Sasaki, Yuji; Tsubata, Yasuhiro; Shirasu, Noriko; Morita, Keisuke; Suzuki, Tomoya
Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1653 - 1656, 2015/09
The concept for the new partitioning method of high-level radioactive waste (HLW) by single-cycle extraction process has been investigated. This process is based on extraction of actinides (An) and fission products (FP), and mutual separation by reverse extraction. Solo extractant and several stripping reagents will be utilized in this process. The extractant employed in this process is required to extract soft (platinum metals), hard acid metals(An), and oxonium anions (Mo, Tc) simultaneously. NTAamide is one of the candidate extractants. After extraction of An and FP by NTAamide(C8), the mutual separation among these metals by reverse extraction will be followed using the suitable water-miscible reagents. The extraction of An and FP, and the masking effect by some water-miscible reagents has been studied.
Suzuki, Tomoya; Shimazaki, Shoma*; Morita, Keisuke; Sasaki, Yuji; Ozawa, Masaki*; Matsumura, Tatsuro
Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1539 - 1543, 2015/09
To understand the adsorption behaviors of ion-exchange resin bearing -trimethylglycine groups (AMP03), adsorption experiments using HNO solutions containing Ru(III), Rh(III), and Pd(II) have been performed. AMP03 strongly adsorbed Pd(II), and Ru(III) and Rh(III) were moderately adsorbed. To control the adsorption abilities of AMP03 for the Ru(III), Rh(III) and Pd(II), adsorption experiments using sample solutions with added thiourea (TU), triethylamine (TEA), and betaine anhydrous were performed. The adsorption abilities for Ru(III) and Rh(III) greatly increased with the addition of TEA, whereas the ability to adsorb Pd(II) was not significantly affected. The addition of TU or betaine anhydrous remarkably decreased the adsorption ability for Pd(II), and contrastingly slight changes in the abilities to adsorb Ru and Rh were also observed. These results show that AMP03 has a significant potential for separation of platinoid elements from HNO solution.
Suzuki, Tomoya; Takao, Koichiro*; Kawasaki, Takeshi*; Harada, Masayuki*; Nogami, Masanobu*; Ikeda, Yasuhisa*
Polyhedron, 96, p.102 - 106, 2015/08
Times Cited Count:5 Percentile:41.5(Chemistry, Inorganic & Nuclear)We have determined crystal structures of UO(NO)() (: 2-imidazolidone), UO(NO)() (: tetrahydro-2-pyrimidone) and UO(NO)() (: 1-methyl-2-imidazolidone) by using single crystal X-ray analysis, and examined correlations between melting points (mps) and intermolecular hydrogen bonds (HBs) of UO(NO)(CU) (CU: cyclic urea derivatives) and UO(NO)(NRP) (NRP: pyrrolidone derivative).
Sasaki, Yuji; Saeki, Morihisa; Sugo, Yumi; Ikeda, Yasuhisa*; Kawasaki, Takeshi*; Suzuki, Tomoya*; Ohashi, Akira*
Solvent Extraction Research and Development, Japan, 22(1), p.37 - 45, 2015/05
Times Cited Count:14 Percentile:42.85(Chemistry, Multidisciplinary)An extractant, methylimino-bis--dioctylacetamide (MIDOA), was used for the extraction of soft acid metals. It was found that MIDOA can extract not only Cr(VI), Mo(VI), W(VI), Tc(VII) and Re(VII), whose metals can form the oxonium anions due to their high oxidation states, but also other metal cations, like Nb(V), Ta(V) and Pd(II). Analogous compounds, imino-bis--dioctylacetamide (IDOA) and methylimino-bis--di-2-ethylhexylacetamide (MIDEHA), are synthesized and compared for their extractability. It is clear that these extractants have almost same or lower values than those for MIDOA. In order to examine the effect on extractability with different donor atoms, TODGA (-tetraoctyl-diglycolamide) and TDGA (-tetraoctyl-tyiodiglycolamide) having oxygen and sulfur donor are employed. The comparison of their extractabilities suggests that the trend of Pd and Re extraction is N S O and N O S, respectively.
Suzuki, Tomoya; Morita, Keisuke; Sasaki, Yuji
Chemistry Letters, 44(2), p.152 - 153, 2015/02
Times Cited Count:2 Percentile:8.3(Chemistry, Multidisciplinary)To recover Rh(III) from HNO solution, adsorption experiments have been performed using an ion-exchange resin bearing an -trimethylglycine group (AMP03). AMP03 was found to exhibit relatively high adsorption ability for Rh(III) for [HNO] 0.02 M ([HNO] denotes HNO concentration in the supernatant), and the values increase significantly with the addition of triethylamine or tris(2-aminoethyl)amine to 0.12 M HNO solutions. In contrast, the addition of thiourea leads to a decrease in the values; i.e., a masking effect on Rh(III) was observed. These results show that AMP03 has a significant potential for effectively recovering Rh from HNO solution.
Sasaki, Yuji; Suzuki, Tomoya; Morita, Keisuke; Tsubata, Yasuhiro
Chemistry Letters, 43(10), p.1538 - 1539, 2014/10
Times Cited Count:6 Percentile:23.1(Chemistry, Multidisciplinary)Several complexing agents including soft donor in their structures are examined for the masking effects of Mo and Re through solvent extraction. The available extractants are hexaoctyl-nitrilotriacetamide (NTAamide) and methyliminodioctylacetamide (MIDOA), whose extractants have high D(Mo, Re). It is clear that Mo and Re in HNO dissolving N-donor ligands, ethylenediamine, diethylenetriamine, and 1,3-diaminopropane, can be suppressed for extraction into organic phase. The ligands including sulfur donor, e.g., thiourea, are also tested, however, less masking effect can be seen.
Sasaki, Yuji; Kitatsuji, Yoshihiro; Sugo, Yumi; Tsubata, Yasuhiro; Suzuki, Tomoya; Kimura, Takaumi; Morita, Yasuji
Proceedings of 20th International Solvent Extraction Conference (ISEC 2014), p.431 - 435, 2014/09
The eight amide extractants including podand-types, which introduce oxygen, nitrogen and sulfur donor atoms in their central frame, are synthesized and their D values for actinide extraction are compared. The central frame affect greatly on their extractability and it is clear that diglycolamide (DGA) has the highest extractability among extractants used here. In addition, DGA having the different length of alkyl chain or phenyl groups attached to amidic N atoms are obtained and the effect of these substituents is studied. Due to the steric hindrance or hydrogen bond, DGA with long and branched alkyl chains, phenyl group, and proton give relatively low D values.